The origin of enhanced O2+ production from photoionized CO2 clusters
Ganguly, Smita LU ; Barreiro, Darío ; Walsh, Noelle LU ; Oostenrijk, Bart LU ; Sorensen, Stacey L LU ; Díaz-Tendero, Sergio and Gisselbrecht, Mathieu LU
(2022)
In Communications Chemistry
- Abstract
- CO2-rich planetary atmospheres are continuously exposed to ionising radiation driving major photochemical processes. In the Martian atmosphere, CO2 clusters are predicted to exist at high altitudes motivating a deeper understanding of their photochemistry. In this joint experimental-theoretical study, we investigate the photoreactions of CO2 clusters (≤2 nm) induced by soft X-ray ionisation. We observe dramatically enhanced production of O2- from photoionized CO2 clusters compared to the case of the isolated molecule and identify two relevant reactions. Using quantum chemistry calculations and multi-coincidence mass spectrometry, we pinpoint the origin of this enhancement: A size-dependent structural transition of the clusters from a... (More)
- CO2-rich planetary atmospheres are continuously exposed to ionising radiation driving major photochemical processes. In the Martian atmosphere, CO2 clusters are predicted to exist at high altitudes motivating a deeper understanding of their photochemistry. In this joint experimental-theoretical study, we investigate the photoreactions of CO2 clusters (≤2 nm) induced by soft X-ray ionisation. We observe dramatically enhanced production of O2- from photoionized CO2 clusters compared to the case of the isolated molecule and identify two relevant reactions. Using quantum chemistry calculations and multi-coincidence mass spectrometry, we pinpoint the origin of this enhancement: A size-dependent structural transition of the clusters from a covalently bonded arrangement to a weakly bonded polyhedral geometry that activates an exothermic reaction producing O+2. Our results unambiguously demonstrate that the photochemistry of small clusters/particles will likely have a strong influence on the ion balance in atmospheres. (Less)
Please use this url to cite or link to this publication:
https://lup.lub.lu.se/record/6777890a-9b2d-4714-9fc0-14d81acb3ca2
- author
- Ganguly, Smita
LU
; Barreiro, Darío
; Walsh, Noelle
LU
; Oostenrijk, Bart
LU
; Sorensen, Stacey L
LU
; Díaz-Tendero, Sergio
and Gisselbrecht, Mathieu
LU
- organization
- publishing date
- 2022-02-04
- type
- Contribution to journal
- publication status
- published
- subject
- in
- Communications Chemistry
- publisher
- Springer Nature
- external identifiers
-
- scopus:85124393595
- ISSN
- 2399-3669
- project
- Studying photodissociation of core ionised CO2 clusters using ion-momentum imaging
- language
- English
- LU publication?
- yes
- id
- 6777890a-9b2d-4714-9fc0-14d81acb3ca2
- alternative location
- https://www.nature.com/articles/s42004-022-00629-z
- date added to LUP
- 2022-02-05 00:39:44
- date last changed
- 2023-04-07 00:39:06
@article{6777890a-9b2d-4714-9fc0-14d81acb3ca2,
abstract = {{CO2-rich planetary atmospheres are continuously exposed to ionising radiation driving major photochemical processes. In the Martian atmosphere, CO2 clusters are predicted to exist at high altitudes motivating a deeper understanding of their photochemistry. In this joint experimental-theoretical study, we investigate the photoreactions of CO2 clusters (≤2 nm) induced by soft X-ray ionisation. We observe dramatically enhanced production of O2- from photoionized CO2 clusters compared to the case of the isolated molecule and identify two relevant reactions. Using quantum chemistry calculations and multi-coincidence mass spectrometry, we pinpoint the origin of this enhancement: A size-dependent structural transition of the clusters from a covalently bonded arrangement to a weakly bonded polyhedral geometry that activates an exothermic reaction producing O+2. Our results unambiguously demonstrate that the photochemistry of small clusters/particles will likely have a strong influence on the ion balance in atmospheres.}},
author = {{Ganguly, Smita and Barreiro, Darío and Walsh, Noelle and Oostenrijk, Bart and Sorensen, Stacey L and Díaz-Tendero, Sergio and Gisselbrecht, Mathieu}},
issn = {{2399-3669}},
language = {{eng}},
month = {{02}},
publisher = {{Springer Nature}},
series = {{Communications Chemistry}},
title = {{The origin of enhanced O2+ production from photoionized CO2 clusters}},
url = {{https://www.nature.com/articles/s42004-022-00629-z}},
year = {{2022}},
}